Method of and apparatus for sputtering, and integrated circuit device

ABSTRACT

A thin film forming method and apparatus, wherein a negative voltage is applied alternately to a target and a substrate to perform film formation and reverse sputter alternately. Further, a coil is mounted between the target and the substrate and a high frequency current is made to flow therethrough to generate plasma. A negative base voltage smaller in absolute value than that during sputter may be applied to the substrate to make Ar ions flow into the substrate while it is subjected to reverse sputter. Thus, a film whose step coverage is 0.3 or more is possible. It becomes also possible to maintain a stable discharge and perform reverse sputter in a high vacuum region. The pressure of an Ar atmosphere may be lowered to 10 -3  Torr or less. An aluminum wiring film whose peak value of x-ray diffraction strength at a (111) plane is 150 Kcps or more is possible. Also, a barrier layer having a layered structure of granular and columnar crystals or a mixed structure thereof providing an efficient barrier effect and a large specific resistance is possible.

This application is a division of application Ser. No. 213,136 filed Jun. 29, 1988, now U.S. Pat. No. 4,999,096.

BACKGROUND OF THE INVENTION

1. Field of the Invention

The present invention relates to a method of and apparatus for forming a thin film through ion impact, and to circuit devices having such a thin film. The invention is particularly suitable for application to barrier layers or wiring films of large scale integrated circuits.

2. Description of the Prior Art

As the density of integration in large scale integrated circuits (LSIs) or very large scale integrated circuits (VLSIs) becomes high, the diameters of contact holes between a silicon substrate and an aluminum wiring film and of through holes between aluminum wiring layers become small, resulting in a larger aspect ratio as shown in FIG. 21. With a magnetron sputter method commonly used in the art, as the aspect ratio becomes near 1, the step coverage shown in FIG. 21 becomes poor due to the shadowing effect during sputter deposition of wiring material, so that wiring failure due to an increase in wiring resistance or electromigration may occur. To eliminate such disadvantages, a bias sputter method, as disclosed in Japanese Patent Unexamined Publication JP-A-61-261472 (corresponding to EP-A-202572) and Japanese Patent Unexamined Publication JP-A-61-214174 (no corresponding foreign application), has been developed whereby a film is formed while applying negative voltages to a target and a substrate at all times. The principle of a DC magnetron bias sputter method is exemplarily shown in FIG. 16. A sputter DC power source 12 is connected to a target 6, while a bias (reverse sputter) DC power source 11 is connected to a substrate 8. These negative electrodes are always supplied with DC negative voltages as shown in FIG. 17 during film formation so that a film is formed while the substrate 8 is being subjected to Ar ion impact (reverse sputter). Therefore, the step coverage is improved as compared with the sputter method employing no bias voltage. In FIG. 16, reference numeral 7 denotes magnets, 10 insulators, 17 a vacuum chamber.

However, it has been found that the crystal orientation (111) of an aluminum wiring film formed by the bias sputter method becomes considerably degraded. It is known that the orientation of crystalline grains is related to electromigration and stressmigration, and the more the orientation becomes excellent, the more the tolerance against electromigration and stressmigration is improved. It has also been found that the bias sputter method may cause cracks in a barrier layer and an inferior barrier effect.

SUMMARY OF THE INVENTION

It is an object of the present invention to provide a thin film forming method and apparatus capable of improving the step coverage and quality of an aluminum wiring film of integrated circuit devices.

It is another object of the present invention to provide a sputtering or vapor deposition method for practicing the thin film forming method as above.

It is a further object of the present invention to provide an integrated circuit device having a wiring film with an improved film quality and step coverage.

It is still a further object of the present invention to provide an aluminum wiring film for integrated circuit devices.

According to the film forming method of this invention, a negative voltage is applied alternately to a target and a substrate to perform film formation and reverse sputter alternately.

The factors affecting the orientation of crystalline grains are residual impurity gasses such as O₂, N₂, H₂ O and the like residual in a vacuum chamber. In admixture of impurity gasses into sputter particles produces crystalline nuclei with different crystal orientations and deposition defects during a growth process, to thereby lower the film quality.

FIG. 18 diagrammatically shows a film forming mechanism of a conventional DC magnetron bias sputter method. Since the substrate 8 and the target 6 are always energized by negative voltages as shown in FIGS. 16 and 17, parts of aluminum and impurities deposited on the substrate are subjected to reverse sputter. Reverse sputtered impurities are dissociated and activated in an atomic state, which impurities are admixed again with aluminum sputter particles from the target, thereby further degrading the film quality. According to the present invention, negative voltages whose waveforms are schematically shown in FIG. 2 are applied alternately to the target and the substrate to solve the above problems. FIGS. 4 and 5 illustrate a film forming mechanism of this invention. Aluminum sputter particles are deposited onto the substrate with a negative voltage being applied to the target. During this process, residual impurity gasses in the vacuum chamber are introduced into the inside of the film on the substrate surface. Next, the voltage applied to the target is turned off and a negative voltage is applied to the substrate, whereby a fraction of the aluminum particles and impurities deposited onto the substrate are subjected to reverse sputter by Ar ion impacts to thereby clean and shape the film. The above processes are alternately and continuously repeated so that a film with a good orientation and step coverage is formed. According to the present invention, a step coverage of 0.3 or more is possible. When a film is formed on a substrate with a recess, the film is substantially parallel to the underneath surface of the substrate at the bottom and side walls of the recess and the upper side surrounding the recess and is inclined at the edge of the recess. The principle idea of this invention has been given above. However, if the sputter and bias voltages are alternately turned off to 0 (set volts), the film forming discharge range is limited. The reason is as follows. As illustrated in the apparatus of this invention shown in FIG. 1, magnets 7 are provided on the target for focussing plasma and enabling sputter discharge at a pressure on the order of 10⁻³ Torr. However, since no magnets are provided on the substrate 8, discharge does not occur even if a negative voltage is applied to the substrate. Thus, the substrate is not subjected to reverse sputter. However, if a coil 5 is mounted between the target 6 and the substrate 8 and a high frequency current is made to flow therethrough to generate plasma, then it becomes possible to maintain a stable discharge and effect reverse sputter in a high vacuum region. According to the present invention, the pressure of the Ar atmosphere may be lowered to 10⁻³ Torr or less. Accordingly, discharge between the target 6 and the electrically grounded vacuum chamber 17 completely stops, and discharge between the substrate and the grounded vacuum chamber can be effected if the substrate is energized to some voltage level. Under certain film forming conditions, the discharge (bias current) may become insufficient. In such a case, according to the present invention, as seen from the waveforms shown in FIG. 3, after a negative voltage is switched from the target to the substrate, sputter discharge is caused to continue by applying a negative base voltage (power) smaller in absolute magnitude than that during sputter (during film forming), to the substrate without making it zero. As a result, Ar ions flow into the substrate which is then subjected to reverse sputter. If the absolute value of this base voltage is made too high, the amount of impurities reintroduced into the film becomes large so that an optimum absolute value of the base voltage must be determined. In addition to the above factors, other factors such as a switching period, a conduction ratio of bias to sputter and the like are selected properly to greatly improve the film characteristic and step coverage.

It is preferable to use a DC bias switching sputter in case of a conductive metal film, and to use a high frequency bias switching sputter in case of an insulating film.

According to a sputter method of this invention, it is possible to set the pressure of Ar gas within a vacuum chamber at 10³¹ 3 Torr or less. Therefore, an admixture of impurities contained in the atmosphere such as O₂, N₂, H₂ O or the like into the film can be suppressed to accordingly obtain a good film quality. If the film forming method of this invention is applied to forming an aluminum wiring film of an integrated circuit device, it is possible to obtain a film whose peak value of x-ray diffraction strength in the (111) plane is 150 Kcps or more, and whose step coverage is 0.3 or more. By virtue of these characteristics, the possibility of a wiring breakage due to electromigration decrease.

The effect of preventing the occurrence of electromigration of a wiring film can be enjoyed obtained not only for pure aluminum wiring films but also for all Al alloy wiring films such as Al-Cu-Si alloy wiring films, Al-Pd-Si alloy wiring films, and Al-Si alloy wiring films. Not only pure aluminum but also Al alloy may be used accordingly as a wiring film of an integrated circuit device.

If the film forming method of this invention is applied to a barrier layer of an integrated circuit device, the resultant barrier layer has a layered structure of granular and columnar crystals or a mixed structure thereof so that it has an efficient barrier effect and a large specific resistance.

The material of the barrier layer is preferably TiN and TiW, however the invention is not limited thereto.

The film forming method of this invention is applicable not only to an integrated circuit device but also to all the devices where a conductive film or an insulating film is formed on a substrate.

According to the film forming method of this invention, it is preferable to ground a vacuum chamber and apply negative pulse voltages alternately to both a target and a substrate.

It is also preferable to set the peak value of a pulse applied to the target higher than the peak value of a pulse applied to the substrate.

It is preferable to set the time during which a negative pulse voltage is applied to the target longer than that during which a negative pulse voltage is applied to the substrate.

It is further preferable to set the base voltage to the target higher than that to the substrate.

BRIEF DESCRIPTION OF THE DRAWINGS

FIG. 1 is a schematic block diagram showing the structure of an embodiment of a thin film forming apparatus according to the present invention;

FIGS. 2 and 3 show examples of waveforms used in the apparatus shown in FIG. 1;

FIGS. 4 and 5 illustrate a film forming mechanism according to the present invention;

FIG. 6 is a characteristic curve illustrating a discharge limit pressure;

FIGS. 7 and 8 are characteristic curves of an x-ray diffraction strength relative to switching factors;

FIG. 9 is a characteristic line of a breakage time relative to an x-ray diffraction strength;

FIG. 10 is a characteristic curve of step coverage relative to a bias ratio;

FIG. 11 shows examples of high frequency waveforms used for sputter and bias;

FIG. 12 schematically illustrates the structure of a TiN film formed according to this invention;

FIG. 13 is a schematic block diagram showing the structure of another embodiment of a thin film forming apparatus according to the present invention;

FIG. 14 shows examples of waveforms used in the apparatus shown in FIG. 13;

FIG. 15 is a schematic block diagram showing the structure of a still further embodiment of a thin film forming apparatus according to the present invention;

FIG. 16 shows the structure of a conventional DC magnetron bias sputter apparatus;

FIG. 17 shows examples of waveforms used in the apparatus shown in FIG. 16;

FIG. 18 illustrates a film forming mechanism associated with FIGS. 16 and 17;

FIG. 19 is a diagrammatical view of the structure of a TiN film formed by a conventional DC magnetron bias sputter method;

FIG. 20 is a diagrammatical view of the structure of a TiN film formed by a conventional DC magnetron sputter method without bias;

FIG. 21 is a view used for explaining an aspect ratio and step coverage;

FIG. 22 shows characteristic curves of an Ar atmospheric pressure relative to an x-ray diffraction strength during the forming of an Al film; and

FIG. 23 is a partial sectional view of an integrated circuit device which shows one of applications of this invention.

DESCRIPTION OF THE PREFERRED EMBODIMENTS Example 1

Referring to FIGS. 1 to 3, an embodiment of a thin film forming apparatus according to the present invention will be described. FIG. 3 diagrammatically shows waveforms used in the apparatus. In FIG. 3, PW denotes a sputter peak power (voltage), BW a sputter base power (voltage), PV a bias peak voltage, BV a bias base voltage, BW/PW a sputter base power ratio, T2/(T1+T2) a bias ratio, and (T1+T2) a switching period. Referring to FIG. 1, the thin film forming apparatus comprises a waveform-controlled sputter power source 2, a constant-voltage waveform-controlled reverse sputter power source 1, a bias current detecting sensor 4, a high frequency coil 5 for generating plasma, a bias current controlling high frequency power source 3 for controlling a bias current and enabling a stable discharge in a high vacuum region, a vacuum chamber 17 within which a film is formed, a substrate (e.g., a Si substrate) 8, a target 6, insulators 10, and an optional waveform generator 9 constituted by a CPU and the like for setting sputter power, bias voltage and current waveforms under program control.

With the thin film forming apparatus constructed as above, first the optional waveform generator 9 sets the sputter power waveform, bias (reverse sputter) waveform and bias current. These signals set by the optional waveform generator 9 are supplied to the waveform controlled sputter power source 2, constant-voltage waveform controlled reverse sputter power source 1 and bias current controlling high frequency power source 3. These power sources have feedback functions to maintain the waveforms as set, even during load variations or the like. Therefore, a change in any one set value will not affect the other values. A bias current control method which is one of the features of this invention will be described in detail. A bias current with the bias voltage PV set, e.g., at 150 V changes if for example a sputter power is changed. To avoid this, a bias current is detected by the bias current detecting sensor 4 and compared with a signal set by the optional waveform generator 9. Based on this comparison, the bias current is maintained at the set value by controlling a high frequency power supplied to the high frequency coil 5 by means of the bias current controlling high frequency power source 3. These operations serve to maintain a stable discharge in a high vacuum region.

Next, explanation will be made of forming a thin film with the thin film forming apparatus shown in FIG. 1 with reference to FIGS. 6 to 10. The thin film formation described below was performed under the conditions that a target was an Al-l weight % Si alloy, a substrate was a Si wafer, an attained vacuum pressure was 3×10⁻⁷ Torr, and a discharge pressure was 5×10⁻⁴ Torr under an Ar atmosphere. The relation between a high frequency power (to be supplied to the coil) and an Ar atmospheric pressure, with respect to continuation of sputter discharge, is shown in FIG. 6 wherein a sputter power was set constant at 500 watts and a high frequency power supplied to the coil was varied over the range of 0 to 200 Watts. The discharge limit pressure at a high frequency power of 0 watt was 9×10⁻⁴ Torr. However, as the high frequency power increased, the discharge limit pressure decreased. With the high frequency power at about 100 watts, the discharge limit pressure decreased slightly and remained substantially constant. For the high frequency power over 100 watts, the discharge limit pressure remained at about 8×10⁻⁵ Torr. As can be seen from the above, discharge according to this invention can be performed in a vacuum region ten times or more higher than that of a conventional DC magnetron sputter method, thus improving a film quality. The high frequency power is preferably in a range of 100 to 200 watts as seen from FIG. 6.

FIG. 7 shows the experimental result of studying the influence of a sputter base power ratio on an x-ray diffraction strength of a film at a (111) orientation, under the conditions that a switching period (T1+T2) was 1 second, a bias peak voltage PV was 150 V, a bias base voltage BV was 50 V, a bias current was 0.3 A, and a sputter base power ratio (BW/PW) was changed from 0 to 1. An x-ray diffraction strength of 370 Kcps was obtained at a sputter base power ratio of about 0 to 0.3. At a larger sputter base power ratio, the diffraction strength considerably deceased to the extent that the strength was 130 Kcps at a sputter base power ratio of 1. The reason why the x-ray diffraction strength is decreased as the sputter base power ratio approaches 1 is that since the sputter power undergoes continuous discharge in a manner similar to that in a conventional method, impurity gases (N₂, O₂, H.sub. 2 O) are introduced into the inside of the film. The diffraction strength was 8 Kcps with a conventional method under the same conditions as above. It should be noted that the diffraction strength according to this invention was about fifty times as high as the conventional strength. The sputter base power ratio is preferably 0.8 or less, and more preferably 0.3 or less.

FIG. 8 shows the experimental result of studying the influence of a switching period upon a diffraction strength, with under the conditions that a sputter base power ratio was 0.3 so as to obtain the maximum diffraction strength as shown in FIG. 7, and a switching period (T1+T2) was changed from 0.1 to 100 seconds. The x-ray diffraction strength was maintained substantially constant within the range of 0.1 to 10 seconds of the switching period, and considerably decreased at the period of 100 seconds. As can be appreciated, the switching period also becomes one of the important film formation factors so that it is necessary to change it in accordance the material and the application field.

FIG. 9 shows the experimental result of studying influence of an x-ray diffraction strength at a (111) orientation plane upon a wiring breakage due to electromigration. An Al-1 weight % Si alloy with a thickness of 0.5 microns was formed on a Si substrate and thereafter a 2 mm long, 0.8 micron wide stripe pattern was formed thereon, and annealed at 450° C. for 60 minutes. A 1 μm thick passivation SiO₂ film was formed thereon by a CVD method. A time was measured until the wiring was broken at a current density of 2×10⁶ A/cm² and under a temperature of 150° C. As can be seen from FIG. 9, it can be understood that as the x-ray diffraction strength increased from 8 to 370 Kcps, the breakage time considerably increased from 40 to 510 hours, thus indicating a certain correlation between the x-ray diffraction strength (orientation) and the electromigration resistance. The diffraction strength of a film formed by means of a conventional DC magnetron sputter method was 8 Kcps as shown in FIG. 9. The wiring breakage time of this film was 40 hours, whereas the film formed by this invention with a maximum diffraction strength of 370 Kcps exhibits a breakage time of 510 hours. Accordingly, the migration resistance of this invention was improved about 14 times over the conventional method.

FIG. 10 shows the result of studying the influence of a bias ratio (T2/(T1+T2)) upon step coverage. Under the conditions that a switching period (T1+T2) was 1 second, a sputter base power ratio (BW/PW) was 0.3, and a bias peak voltage (PV) was 150 V, a pattern having a through hole diameter of 0.8 micron and an aspect ratio of 1 was formed on an Si substrate, and a film of Al-l weight % Si alloy was formed thereon to study the step coverage state by using a scanning microwave spectrometer. The step coverage presented a maximum value 60% at a bias ratio of 0.3, and it decreased at a ratio above and below 0.3. As can be seen from the film configuration at the through hole sections shown in FIG. 10, the film configuration varies with the bias ratio. For instance, it was possible to further improve the step coverage by setting the bias ratio to be large at the start of film formation and lowering it with time. The step coverage of a film formed by a conventional DC magnetron bias sputter method under the same bias voltage 150 V as of the present invention was 22%. The film configuration can be varied with the bias ratio according to the present invention. However, the conventional method fixes the bias voltage and no other factors remain so that the step coverage cannot be improved. With the conventional method, if the bias voltage is increased, the kinetic energy of ions increases so that the step coverage can be improved more or less. However, in this case, ion impact may damage the substrate and the film quality is greatly degraded.

FIG. 22 shows the results of comparing various conventional methods with the method of this invention with respect to the influence of an Ar atmospheric pressure upon the x-ray diffraction strength at a (111) orientation of an Al film formed on an Si substrate, wherein the apparatus shown in FIG. 1 was used for the film formation of this invention.

The film formation of this invention was made under the conditions that a switching period of sputtering relative to reverse sputtering was 1 second, a bias peak voltage was 150 V, a bias ratio was 0.3, and a sputter base power ratio was 0.3.

For those conventional methods shown in FIG. 22, the sputter method is a method that does not include reverse sputter, the bias sputter method is a method in which sputtering is carried out while a negative voltage is applied to a substrate, and the waveform controlled AC sputter method, as described in Japanese Patent Application No. 61-169590 (unexamined publication JP-A-63-26361), is a method in which sputtering is carried out using an AC voltage whose waveform is controlled. With the method of this invention, film formation can be carried out at a pressure lower than 10⁻³ Torr so that the x-ray diffraction strength can be made considerably higher than in a conventional method.

In contrast, the conventional methods can not be used at the an Ar atmospheric pressure lower than 10⁻³ Torr and the x-ray diffraction strength is limited to 100 Kcps at most. The method of this invention is the first to succeed in making the x-ray diffraction strength of an Al film at a (111) plane higher than 150 Kcps.

Example 2

The DC sputter of Example 1 is effective for conductive targets, but a target of insulating material cannot be discharged. In Example 2, the waveform controlled sputter power source 2 and the constant-voltage waveform controlled reverse sputter power source 1 shown in FIG. 1 were replaced with high frequency power sources having frequencies of about 13.5 MHz having waveforms as shown in the schematic diagram of FIG. 11, thereby allowing discharge of a target of insulating material. An Al film was formed and patterned in the manner described in Example 1, and thereafter an SiO₂ film corresponding to an inter-layer insulating film of a multi-layered wiring was formed thereon. Contact between step portions was excellent, and the surface unevenness was considerably improved.

Example 3

Contact resistance increases largely for contact holes smaller than 1 micron, because the diameter of Si grains crystallized from an Al wiring film may sometimes exceed 1 micron. One of the methods for preventing this is to use a barrier metal. Various types of barrier metal are known. TiN is the most prominent to prevent reaction between Al and Si. However, a TiN barrier film formed under an (Ar+N₂ +O₂) atmosphere with a Ti target has columnar crystals as shown by a film cross section in FIG. 20. According to the characteristics of this film, it has a small residual stress, no defects such as cracks, and an excellent barrier effect. However, it has the disadvantage of a large specific resistance on the order of 1000 to 2000 μΩ·cm.

On the other hand, a film formed by applying a negative bias (reverse sputter) to a substrate has fine granular crystals as shown in FIG. 19. As compared with the above specific resistance, this film has a very low resistance on the order of 50 to 200 μΩ·cm. However, it has a large residual stress and is likely to generate cracks, and also has a poor barrier effect.

Material having both a small specific resistance and presenting an excellent barrier effect is suitable for a barrier film material. However, in this respect, both the above-described methods are contradictory to each other and present an obstacle to practical use. This has resulted in the consideration that if a film is formed by alternately using sputter and reverse sputter, the film will be a layered film of columnar and granular crystals as shown in FIG. 12 or a mixed film thereof which has both the above-mentioned advantageous features. Accordingly, a film was formed under the conditions that a switching period was 10 seconds, a bias ratio was 0.5, a sputter base power ratio was 0.3, a target was Ti, and an atmosphere was Ar (7.5)+N₂ (2)+O₂ (0.5). The resultant film had a specific resistance on the order of 180 to 250 μΩ·cm. After annealing at 450° C., there was no barrier layer breakage, no crystallization of Si from an Al wiring layer, and no cracks in the film. As above, a composite film can be formed by applying this invention to reactive sputtering.

FIG. 23 shows the structure of an integrated circuit wherein a TiN film was formed on an Si substrate by using the above method, an Al wiring film was formed thereon, and an SiO₂ passivation film was formed over the entire surface of the circuit. The passivation film is also not limited to SiO₂ only. The substrate is not limited to Si, but other materials such as GaAs may be used.

Example 4

In Example 4, a target was arranged like the structure of the apparatus of FIG. 4, and a film was formed by sputtering with the aid of ions generated within the vacuum chamber between the ground potential and the target and substrate potentials. The evaporation source may be activated by an electron beam vapor deposition method, resistance heating vapor deposition method, or high frequency heating vapor deposition method. FIG. 13 shows an example of an electron beam evaporation source. Thermal electrons are generated from a filament 13 and accelerated by means of a waveform-controlled thermal electron acceleration voltage power source 11, and are focused upon an evaporation material 14 to evaporate it by a deflection coil 16. Reference numeral 12 denotes a filament heating power source, and reference numeral 15 denotes a crucible. Film formation is basically performed by the above operation and switching of a voltage applied to the substrate 8. However, even if an electron beam in the form of pulses is applied to the evaporation material 14, the material cannot be evaporated at once due to its thermal inertia. To avoid this, as shown by waveforms of FIG. 14, during the period in which a negative voltage is applied to the substrate for reverse sputter, the electron beam (thermal electron acceleration voltage) is not completely turned off, but a base electron beam is applied. Since the evaporation material is pre-heated by the base electron beam, the response and control of evaporation of the evaporation material 14 can be improved. Further, if the electron beam output waveform from the thermal electron acceleration voltage waveform controlled power source changes, the focus of the electron beam is caused to shift. To avoid this, a voltage to be applied to the deflection coil 16 is synchronized with a thermal electron waveform output (voltage). According to the results of various experiments made with the present apparatus, the x-ray diffraction strength of an Al film at a (111) crystal grain orientation was reduced to 30% of Example 1, and the film forming speed was three times as fast as that of Example 1.

Example 5

In Example 5 shown in FIG. 15, an ion source for ion impact upon a target 6 and another ion source for ion impact upon a substrate are separately provided, and both the ion sources are alternately switched to form a film and perform a reverse sputter. The ion source may be activated by a microwave method, a high frequency method, or a thermal electron method. FIG. 15 shows an example of a microwave ion source. Waveform-shaped microwaves generated by waveform controlled microwave power sources 19 in accordance with signals from an optional waveform generator 9 are guided to plasma generating chambers 24 via waveguides 22 to generate plasma. Each of the plasma generating chambers 24 is provided with a mesh ion deriving electrode 21 to which a negative voltage is applied from waveform controlled ion deriving power sources 20 to derive ions within a vacuum chamber 17. The ion sources are alternately switched to impinge ions onto the target and substrate to thereby form a film and perform a reverse sputter. A characteristic feature of this method resides in the ion energy can be changed as desired by changing the microwave output or the ion deriving voltage. In addition, since the ion sources are separately provided, there is no interference therebetween. Further, the film forming chamber and the ion sources are separated by the mesh electrodes so that a film can be formed in a vacuum region as high as 10 to 100 times as that at the ion sources. As a result, an adequate vacuum region is broad and the film quality is superior to Example 1. However, the film forming speed was reduced to 40% of Example 1.

As described so far, ion impacts (reverse sputter) are alternately switched to form a film so that the orientation of crystal grains and step coverage can be considerably improved. Further, good orientation results in high tolerance against electromigration so that the lifetime of Al or Al alloy wiring films on VLSIs can be prolonged, and reliability can be extensively improved. Such an improved step coverage is not only compatible with future wiring processes of VLSIs under continual miniatuarization, but also can improve the reliability of present VLSIs. Furthermore, film formation under a reactive gas atmosphere produces a composite film with excellent characteristics which can not be attained by a conventional sputter method and a conventional bias sputter method. 

We claim:
 1. An integrated circuit device having a barrier layer which is interposed between an aluminum wiring film and a semiconductor substrate of an integrated circuit, said barrier layer having a layered structure of alternating sublayers of granular and columnar crystals.
 2. An integrated circuit device according to claim 1, wherein a peak value of an x-ray diffraction strength of said aluminum wiring film at a (111) plane of said aluminum wiring film is 150 Kcps or more.
 3. An integrated circuit device according to claim 1, wherein said barrier is made of TiN.
 4. An aluminum wiring film formed on a substrate wherein a peak value of an x-ray diffraction strength at a (111) plane of said aluminum wiring film is 150 Kcps or more.
 5. An article comprising one of a sputtered film and a vapor-deposited film, the film being formed on a substrate such that the film has a layered structure of granular and columnar crystals. 